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Here, using first-principles calculations, we show that monoclinic BaIn2As2 undergoes two successive pressure-driven topological phase transitions within the same P2\/m structural phase, evolving from a topological insulator at ambient pressure to a trivial insulator at 16 GPa and then to a high-pressure topological semimetal at 26 GPa. The two nontrivial phases share the same Z2 = 1 classification but exhibit distinct surface spectra and opposite low-energy optical anisotropy. We establish a two-level identification scheme in which spin Hall conductivity provides a fingerprint for separating nontrivial phases from the trivial phase, with possible inverse spin Hall electrical readout, whereas monoclinic symmetry-enabled in-plane reflectance anisotropy resolves the two nontrivial phases. We further propose a diamond-anvil-cell platform combining yttrium-iron-garnet-based spin pumping with polarization-resolved infrared reflectance.<\/jats:p>","DOI":"10.1021\/acsomega.6c07032","type":"journal-article","created":{"date-parts":[[2026,9,10]],"date-time":"2026-09-10T08:01:15Z","timestamp":1789027275000},"page":"56265-56271","source":"Crossref","is-referenced-by-count":0,"title":["Spin and Optical Fingerprints of Pressure-Driven Double\nTopological Phase Transition in Monoclinic BaIn2As2"],"prefix":"10.1021","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0016-8930","authenticated-orcid":true,"given":"Wen-Ti","family":"Guo","sequence":"first","affiliation":[{"name":"Fujian Normal University , , ,","place":["Fuzhou, China, 350117"]},{"name":"Nanjing University , , ,","place":["Nanjing, China, 210093"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0356-5387","authenticated-orcid":true,"given":"Jian-Min","family":"Zhang","sequence":"additional","affiliation":[{"name":"Fujian Normal University , , ,","place":["Fuzhou, China, 350117"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,10]]},"reference":[{"key":"2026092211022265100_cit1","doi-asserted-by":"publisher","first-page":"146802","DOI":"10.1103\/PhysRevLett.95.146802","article-title":"Topological Order and the Quantum Spin Hall Effect","volume":"95","author":"Kane","year":"2005","journal-title":"Phys. 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